The methods described herein provide self-assembling macromolecular networks within the human skin. The methods provide instant and accumulation-based physical properties within the skin, causing cosmetic benefits including, bulking/plumping, filling, strengthening, smoothing, firming, and lifting, as well as enhancing the optical properties, radiance and other cosmetic appearance characteristics of the skin. The disclosure also provides a method of re-structuring the skin without cellular biogenesis by effecting macrostructures within the skin. The method comprising effectuating self-assembly within the skin layers by topically applying a composition comprising at least one self-assembly material to form functional macrostructures within the skin and effectuating self-assembly of the at least one self-assembly material in vivo while substantially preventing self-assembly prior to the topical application or treatment.